非晶态固体的精确电子结构：揭示黑色二氧化钛的颜色起源和颜色
Precise electronic structures of amorphous solids: unraveling the color origin and photocatalysis of black titania
摘要：
通过高效催化剂分解水是40年内实现碳中和的最终解决方案。为了实现这一目标，非晶态光催化剂以其有前途的性能而闻名。其中，最著名的是黑二氧化钛（无定形TiOx，x < 2）。然而，尽管对黑色二氧化钛进行了大量的研究，但其颜色来源，结构-性质关系和光催化机理仍然是一个热门争论的话题，主要是由于难以计算其精确的电子结构。在这里，使用从头算分子动力学模拟，我们报告了黑二氧化钛的精确的电子结构，并进一步揭示了共价化合物的电子结构的非晶化和还原后的一般演化模式。此外，助催化剂原子的表面吸附（例如，Pt）在非晶态物质上的表面：无序的表面使助催化剂原子易于容纳，而扩展的电子态有利于光生电子和空穴的分离，有利于析氢。该研究阐明了非晶态催化剂的工作原理，并为提高其性能提供了实际指导。
英文摘要：
Water splitting through efficient catalysts represents an ultimate solution for carbon neutrality within 40 years. To achieve this goal, amorphous photocatalysts are noted for their promising performances. Among them, the best known is black titania (amorphous TiOx, x < 2). However, despite the large number of studies on black titania, its color origin, structure-property relationship, and photocatalytic mechanism remain a topic of hot debate, largely due to the difficulty to calculate its precise electronic structure. Here, using ab initio molecular dynamics simulations, we report the precise electronic structures of black titania and further reveal the generic evolution pattern of the electronic structures of covalent compounds upon amorphization and reduction. Moreover, surface adsorption of the co-catalyst atoms (e.g., Pt) on amorphous substances is simulated for the first time: the disordered surface enables easy accommodation of the co-catalyst atoms, while the extended electronic states facilitate the separation of photo-induced electrons and holes, beneficial for hydrogen evolution. This study elucidates the workings of amorphous catalysts and offers practical guidance for enhancing their performances.
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